In 2002, the National Science Foundation established the Network for Computational Nanotechnology (NCN), a network of universities supporting the National Nanotechnology Initiative by bringing computational tools online, making the tools easy to use, and supporting the tools with educational materials. Along the way, NCN created a unique cyberinfrastructure to support its Web site, nanoHUB.org, where researchers, educators, and professionals collaborate, share resources, and solve real nanotechnology problems. In 2007, nanoHUB.org served more than 56,000 users from 172 countries. In this article, the authors share their experiences in developing this cyberinfrastructure and using it, particularly in an educational context.